The sustainable production of green hydrogen via water electrolysis necessitates cost-effective electrocatalysts.By following the circular economy principle,the utilization of waste-derived catalysts significantly pro...The sustainable production of green hydrogen via water electrolysis necessitates cost-effective electrocatalysts.By following the circular economy principle,the utilization of waste-derived catalysts significantly promotes the sustainable development of green hydrogen energy.Currently,diverse waste-derived catalysts have exhibited excellent catalytic performance toward hydrogen evolution reaction(HER),oxygen evolution reaction(OER),and overall water electrolysis(OWE).Herein,we systematically examine recent achievements in waste-derived electrocatalysts for water electrolysis.The general principles of water electrolysis and design principles of efficient electrocatalysts are discussed,followed by the illustration of current strategies for transforming wastes into electrocatalysts.Then,applications of waste-derived catalysts(i.e.,carbon-based catalysts,transitional metal-based catalysts,and carbon-based heterostructure catalysts)in HER,OER,and OWE are reviewed successively.An emphasis is put on correlating the catalysts’structure-performance relationship.Also,challenges and research directions in this booming field are finally highlighted.This review would provide useful insights into the design,synthesis,and applications of waste-derived electrocatalysts,and thus accelerate the development of the circular economy-driven green hydrogen energy scheme.展开更多
Tuning the surface properties of catalysts is an effective method for accelerating water electrolysis.Herein,we propose a directional doping and interfacial coupling strategy to design two surface-functionalized Schot...Tuning the surface properties of catalysts is an effective method for accelerating water electrolysis.Herein,we propose a directional doping and interfacial coupling strategy to design two surface-functionalized Schottky junction catalysts for coordinating the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Directional doping with B/S atoms endows amphiphilic g-C_(3)N_(4)with significant n-/p-type semiconductor properties.Further coupling with Fe_(3)C modulates the energy band levels of B-C_(3)N_(4)and S-C_(3)N_(4),thus resulting in functionalized Schottky junction catalysts with specific surface-adsorption properties.The space-charge region generated by the dual modulation induces a local“OH-and Ht-enriched”environment,thus selectively promoting the kinetic behavior of the OER/HER.Impressively,the designed B-C_(3)N_(4)@Fe_(3)C||S-C_(3)N_(4)@Fe_(3)C pair requires only a low voltage of 1.52 V to achieve efficient water electrolysis at 10 mA cm^(-2).This work highlights the potential of functionalized Schottky junction catalysts for coordinating redox reactions in water electrolysis,thereby resolving the trade-off between catalytic activity and stability.展开更多
Mixed ionic-electronic conductors(MIECs)play a crucial role in the landscape of energy conversion and storage technologies,with a pronounced focus on electrode materials’application in solid oxide fuel cells(SOFCs)an...Mixed ionic-electronic conductors(MIECs)play a crucial role in the landscape of energy conversion and storage technologies,with a pronounced focus on electrode materials’application in solid oxide fuel cells(SOFCs)and proton-conducting ceramic fuel cells(PCFCs).In parallel,the emergence of semiconductor ionic materials(SIMs)has introduced a new paradigm in the field of functional materials,particularly for both electrode and electrolyte development for low-temperature,300–550℃,SOFCs,and PCFCs.This review article critically delves into the intricate mechanisms underpinning the synergistic relationship between MIECs and SIMs,with a particular emphasis on elucidating the fundamental working principles of semiconductor ionic membrane fuel cells(SIMFCs).By exploring critical facets such as ion-coupled electron transfer/transport,junction effect,energy bands alignment,and theoretical computations,it casts an illuminating spotlight on the transformative potential of MIECs,also involving triple charge conducting oxides(TCOs)in the context of SIMs and advanced fuel cells(FCs).The insights and findings articulated herein contribute substantially to the advancement of SIMs and SIMFCs by tailoring MIECs(TCOs)as promising avenues toward the emergence of high-performance SIMFCs.This scientific quest not only addresses the insistent challenges surrounding efficient charge transfer,ionic transport and power output but also unlocks the profound potential for the widespread commercialization of FC technology.展开更多
Catalytic conversion of biomass-based platform chemicals is one of the significant approaches to utilize renewable biomass resources.2,5-Furandicarboxylic acid(FDCA),obtained by an electrocatalytic oxidation of 5-hydr...Catalytic conversion of biomass-based platform chemicals is one of the significant approaches to utilize renewable biomass resources.2,5-Furandicarboxylic acid(FDCA),obtained by an electrocatalytic oxidation of 5-hydroxymethylfurfural(HMF),has attracted extensive attention due to the potential of replacing terephthalic acid to synthesize high-performance polymeric materials for commercialization.In the present work,the pHdependent reaction pathways and factors influencing the degree of functional group oxidation are first discussed.Then the reaction mechanism of HMF oxidation is further elucidated using the representative examples.In addition,the emerging catalyst design strategies(defects,interface engineering)used in HMF oxidation are generalized,and structure-activity relationships between the abovementioned strategies and catalysts performance are analyzed.Furthermore,cathode pairing reactions,such as hydrogen evolution reaction,CO_(2) reduction reaction(CO_(2)RR),oxygen reduction reaction,and thermodynamically favorable organic reactions to lower the cell voltage of the electrolysis system,are discussed.Finally,the challenges and prospects of the electrochemical oxidation of HMF for FDCA are presented,focusing on deeply investigated reaction mechanism,coupling reaction,reactor design,and downstream product separation/purification.展开更多
Semiconductors and the associated methodologies applied to electrochemistry have recently grown as an emerging field in energy materials and technologies.For example,semiconductor membranes and heterostructure fuel ce...Semiconductors and the associated methodologies applied to electrochemistry have recently grown as an emerging field in energy materials and technologies.For example,semiconductor membranes and heterostructure fuel cells are new technological trend,which differ from the traditional fuel cell electrochemistry principle employing three basic functional components:anode,electrolyte,and cathode.The electrolyte is key to the device performance by providing an ionic charge flow pathway between the anode and cathode while preventing electron passage.In contrast,semiconductors and derived heterostructures with electron(hole)conducting materials have demonstrated to be much better ionic conductors than the conventional ionic electrolytes.The energy band structure and alignment,band bending and built-in electric field are all important elements in this context to realize the necessary fuel cell functionalities.This review further extends to semiconductor-based electrochemical energy conversion and storage,describing their fundamentals and working principles,with the intention of advancing the understanding of the roles of semiconductors and energy bands in electrochemical devices for energy conversion and storage,as well as applications to meet emerging demands widely involved in energy applications,such as photocatalysis/water splitting devices,batteries and solar cells.This review provides new ideas and new solutions to problems beyond the conventional electrochemistry and presents new interdisciplinary approaches to develop clean energy conversion and storage technologies.展开更多
基金supported by the Australian Research Council (ARC) Discovery Project (DP220101139)support of the Australian Research Council (ARC) through Project DE220100530support of the Australian Research Council (ARC) through Project DE200100970
文摘The sustainable production of green hydrogen via water electrolysis necessitates cost-effective electrocatalysts.By following the circular economy principle,the utilization of waste-derived catalysts significantly promotes the sustainable development of green hydrogen energy.Currently,diverse waste-derived catalysts have exhibited excellent catalytic performance toward hydrogen evolution reaction(HER),oxygen evolution reaction(OER),and overall water electrolysis(OWE).Herein,we systematically examine recent achievements in waste-derived electrocatalysts for water electrolysis.The general principles of water electrolysis and design principles of efficient electrocatalysts are discussed,followed by the illustration of current strategies for transforming wastes into electrocatalysts.Then,applications of waste-derived catalysts(i.e.,carbon-based catalysts,transitional metal-based catalysts,and carbon-based heterostructure catalysts)in HER,OER,and OWE are reviewed successively.An emphasis is put on correlating the catalysts’structure-performance relationship.Also,challenges and research directions in this booming field are finally highlighted.This review would provide useful insights into the design,synthesis,and applications of waste-derived electrocatalysts,and thus accelerate the development of the circular economy-driven green hydrogen energy scheme.
基金supported by the National Natural Science Foundation of China(No.51672208)the Key Science and Technology Innovation Team of Shaanxi Province(2022TD-34)Open foundation Project of Key Laboratory of Plateau Green Building and Ecological Community of Qinghai Province(KLKF-2019-002)。
文摘Tuning the surface properties of catalysts is an effective method for accelerating water electrolysis.Herein,we propose a directional doping and interfacial coupling strategy to design two surface-functionalized Schottky junction catalysts for coordinating the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Directional doping with B/S atoms endows amphiphilic g-C_(3)N_(4)with significant n-/p-type semiconductor properties.Further coupling with Fe_(3)C modulates the energy band levels of B-C_(3)N_(4)and S-C_(3)N_(4),thus resulting in functionalized Schottky junction catalysts with specific surface-adsorption properties.The space-charge region generated by the dual modulation induces a local“OH-and Ht-enriched”environment,thus selectively promoting the kinetic behavior of the OER/HER.Impressively,the designed B-C_(3)N_(4)@Fe_(3)C||S-C_(3)N_(4)@Fe_(3)C pair requires only a low voltage of 1.52 V to achieve efficient water electrolysis at 10 mA cm^(-2).This work highlights the potential of functionalized Schottky junction catalysts for coordinating redox reactions in water electrolysis,thereby resolving the trade-off between catalytic activity and stability.
基金supported by the Science and Technology Department of Jiangsu Province under Grant(BE2022029)Jiangsu Provincial Innovation and Entrepreneurship Talent Program(JSSCRC2021491)+3 种基金Key Program for International S&T Cooperation Projects of Shaanxi Province(2019KWZ-03)Key Program for Nature Science Foundation of Shaanxi Province(2019JZ-20)Key Science and Technology Innovation Team of Shaanxi Province(2022TD-34)the Beijing Natural Science Foundation under Grant(IS23050)is greatly acknowledged.
文摘Mixed ionic-electronic conductors(MIECs)play a crucial role in the landscape of energy conversion and storage technologies,with a pronounced focus on electrode materials’application in solid oxide fuel cells(SOFCs)and proton-conducting ceramic fuel cells(PCFCs).In parallel,the emergence of semiconductor ionic materials(SIMs)has introduced a new paradigm in the field of functional materials,particularly for both electrode and electrolyte development for low-temperature,300–550℃,SOFCs,and PCFCs.This review article critically delves into the intricate mechanisms underpinning the synergistic relationship between MIECs and SIMs,with a particular emphasis on elucidating the fundamental working principles of semiconductor ionic membrane fuel cells(SIMFCs).By exploring critical facets such as ion-coupled electron transfer/transport,junction effect,energy bands alignment,and theoretical computations,it casts an illuminating spotlight on the transformative potential of MIECs,also involving triple charge conducting oxides(TCOs)in the context of SIMs and advanced fuel cells(FCs).The insights and findings articulated herein contribute substantially to the advancement of SIMs and SIMFCs by tailoring MIECs(TCOs)as promising avenues toward the emergence of high-performance SIMFCs.This scientific quest not only addresses the insistent challenges surrounding efficient charge transfer,ionic transport and power output but also unlocks the profound potential for the widespread commercialization of FC technology.
基金University of Electronic Science and Technology of China,Grant/Award Number:A1098531023601208Scientific Research Foundation,Grant/Award Number:Y030212059003045+1 种基金China Postdoctoral Science Foundation,Grant/Award Numbers:2021TQ0059,2022M710610National Natural Science Foundation of China,Grant/Award Numbers:21464015,21472235。
文摘Catalytic conversion of biomass-based platform chemicals is one of the significant approaches to utilize renewable biomass resources.2,5-Furandicarboxylic acid(FDCA),obtained by an electrocatalytic oxidation of 5-hydroxymethylfurfural(HMF),has attracted extensive attention due to the potential of replacing terephthalic acid to synthesize high-performance polymeric materials for commercialization.In the present work,the pHdependent reaction pathways and factors influencing the degree of functional group oxidation are first discussed.Then the reaction mechanism of HMF oxidation is further elucidated using the representative examples.In addition,the emerging catalyst design strategies(defects,interface engineering)used in HMF oxidation are generalized,and structure-activity relationships between the abovementioned strategies and catalysts performance are analyzed.Furthermore,cathode pairing reactions,such as hydrogen evolution reaction,CO_(2) reduction reaction(CO_(2)RR),oxygen reduction reaction,and thermodynamically favorable organic reactions to lower the cell voltage of the electrolysis system,are discussed.Finally,the challenges and prospects of the electrochemical oxidation of HMF for FDCA are presented,focusing on deeply investigated reaction mechanism,coupling reaction,reactor design,and downstream product separation/purification.
基金the National Natural Science Foundation of China(51772080,51672208,51774259,and 51402093)the Natural Science Foundation of Guangdong Province(2021A1515012356 and 2017A030313289)+4 种基金the project foundation from the Ministry of Education of Guangdong Province(2019KTSCX151)Shenzhen Government Plan of Science and Technology(JCYJ20180305125247308)the National Laboratory of Solid State Microstructures,Nanjing University,EPSRC(EP/I013229/1)Royal Society and Newton Fund(NAF\R1\191294)Key Program for International S&T Cooperation Projects of Shaanxi Province(2019JZ-20,2019KWZ-03)。
文摘Semiconductors and the associated methodologies applied to electrochemistry have recently grown as an emerging field in energy materials and technologies.For example,semiconductor membranes and heterostructure fuel cells are new technological trend,which differ from the traditional fuel cell electrochemistry principle employing three basic functional components:anode,electrolyte,and cathode.The electrolyte is key to the device performance by providing an ionic charge flow pathway between the anode and cathode while preventing electron passage.In contrast,semiconductors and derived heterostructures with electron(hole)conducting materials have demonstrated to be much better ionic conductors than the conventional ionic electrolytes.The energy band structure and alignment,band bending and built-in electric field are all important elements in this context to realize the necessary fuel cell functionalities.This review further extends to semiconductor-based electrochemical energy conversion and storage,describing their fundamentals and working principles,with the intention of advancing the understanding of the roles of semiconductors and energy bands in electrochemical devices for energy conversion and storage,as well as applications to meet emerging demands widely involved in energy applications,such as photocatalysis/water splitting devices,batteries and solar cells.This review provides new ideas and new solutions to problems beyond the conventional electrochemistry and presents new interdisciplinary approaches to develop clean energy conversion and storage technologies.
